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Physical review. B./Physical review. B

Excited-state lifetime of the NV− infrared transition in diamond

Ronald Ulbricht, Zhi-Heng Loh

Published Sep 28, 2018• 33 citations
Publisher

Abstract

The negatively charged nitrogen vacancy ($\mathrm{N}{\mathrm{V}}^{\ensuremath{-}}$) defect in diamond serves as a popular platform for manipulating and exploiting long-lived coherent spin dynamics at room temperature combined with optical readout. The required spin polarization of the spin triplet $^{3}A_{2}$ electronic ground state occurs through a cycle of repetitious optical photoexcitation events to the $^{3}E$ electronic excited state that is accompanied by a series of electronic transitions to a $^{1}A_{1}$ and a $^{1}E$ electronic state, and back to the $^{3}A_{2}$ state. The timescales of these transitions are largely known, yet for the relaxation time of the $^{1}A_{1}\ensuremath{\rightarrow}^{1}E$ infrared transition, which predominantly occurs via nonradiative recombination, only an upper limit of 1 ns could be determined so far. Here, we employ ultrafast transient absorption spectroscopy to probe the dynamics of the nonradiative relaxation from the $^{1}A_{1}$ to the $^{1}E$ state after photoexcitation of the $^{3}E$ state and find a relaxation time of 100 ps at a temperature of 78 K.

DOI
10.1103/physrevb.98.094309

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Nitrogen-vacancy (NV) complex in diamond is one of the most prominent solid state defects as the negatively charged NV defect (NV−) is a leading contender for quantum technologies. In quantum information processing applications, NV− is photoexcited that often leads to photoionization to neutral NV defect, NV0, and re-ionization back to NV− should occur to control the S=1 spin of NV−. As a consequence, understanding the photophysics of NV0 is crucial for controlling NV−. Furthermore, recent studies have shown that the S=1/2 electron spin of NV0 can also be initialized and read out at certain conditions that turns single NV0 a potential quantum bit. Quantum optics protocols rest on detailed knowledge on the electronic structure of the given system, which is obviously missing for NV0 in diamond. In this study, we combine the group theory and density functional theory calculations toward exploring the nature of the ground and excited states of NV0. We show that the effective three-electron system of NV0 leads to high correlation effects that make this system very challenging for ab initio simulations.

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The negatively charged nitrogen vacancy (NV\ensuremath−\mathrm{N}{\mathrm{V}}^{\ensuremath{-}}NV\ensuremath−) defect in diamond serves as a popular platform for manipulating and exploiting long-lived coherent spin dynamics at room temperature combined with optical readout. The required spin polarization of the spin triplet 3A2^{3}A_{2}3A2​ electronic ground state occurs through a cycle of repetitious optical photoexcitation events to the 3E^{3}E3E electronic excited state that is accompanied by a series of electronic transitions to a 1A1^{1}A_{1}1A1​ and a 1E^{1}E1E electronic state, and back to the 3A2^{3}A_{2}3A2​ state. The timescales of these transitions are largely known, yet for the relaxation time of the 1A1\ensuremath→1E^{1}A_{1}\ensuremath{\rightarrow}^{1}E1A1​\ensuremath→1E infrared transition, which predominantly occurs via nonradiative recombination, only an upper limit of 1 ns could be determined so far. Here, we employ ultrafast transient absorption spectroscopy to probe the dynamics of the nonradiative relaxation from the 1A1^{1}A_{1}1A1​ to the 1E^{1}E1E state after photoexcitation of the 3E^{3}E3E state and find a relaxation time of 100 ps at a temperature of 78 K.
Abstract Nitrogen-vacancy (NV) defect centers in diamond are key to applications in quantum sensing and quantum computing. They create localized electronic states in the diamond lattice with distinct population relaxation pathways following photoexcitation that ultimately enable its unique properties. The defect is known to exist in two charge states: neutral and negative, with respectively one and two known optically-active electronic transitions. Here, we report on the observation of a large number of hitherto undiscovered excited electronic states in both charge states as evidenced by distinct optical transitions in the infrared to ultraviolet part of the spectrum. These transitions are observed by monitoring the electronic relaxation of NV centers after photoexcitation using transient absorption spectroscopy, directly probing transient phenomena occurring on timescales from femtoseconds to microseconds. We also for the first time probed the electron transfer dynamics from the 3 E state of NV− to nearby single-substitutional nitrogen defects (N s ) that leads to the well-known effect of NV photoluminescence quenching.
We report measurements of the optical properties of the 1042 nm transition of negatively charged nitrogen-vacancy (NV) centers in type-1b diamond. The results indicate that the upper level of this transition couples to the ${m}_{s}=\ifmmode\pm\else\textpm\fi{}1$ sublevels of the 3E^{3}E3E excited state and is short lived with a lifetime of $\ensuremath{\lesssim}1\text{ }\text{ns}$. The lower level is shown to have a temperature-dependent lifetime of 462(10) ns at 4.4 K and 219(3) ns at 295 K. The light-polarization dependence of 1042 nm absorption confirms that the transition is between orbitals of A1{A}_{1}A1​ and EEE character. The results shed light on the NV level structure and optical pumping mechanism.
Negatively charged nitrogen-vacancy (NV${}^{\ensuremath{-}}$) color centers in diamond have generated much interest for use in quantum technology. Despite the progress made in developing their applications, many questions about the basic properties of NV${}^{\ensuremath{-}}$ centers remain unresolved. Understanding these properties can validate theoretical models of NV${}^{\ensuremath{-}}$, improve their use in applications, and support their development into competitive quantum devices. In particular, knowledge of the phonon modes of the 1A1{}^{1}{A}_{1}1A1​ electronic state is key for understanding the optical pumping process. Using pump-probe spectroscopy, we measured the phonon sideband of the ${}^{1}E\ensuremath{\rightarrow}{}^{1}{A}_{1}$ electronic transition in the NV${}^{\ensuremath{-}}$ center. From this we calculated the ${}^{1}E\ensuremath{\rightarrow}{}^{1}{A}_{1}$ one-phonon absorption spectrum and found it to differ from that of the ${}^{3}E\ensuremath{\rightarrow}{}^{3}{A}_{2}$ transition, a result which is not anticipated by previous group-theoretical models of the NV${}^{\ensuremath{-}}$ electronic states. We identified a high-energy 169-meV localized phonon mode of the 1A1{}^{1}{A}_{1}1A1​ level.
Spin defects in diamond are promising platforms for quantum sensing. The longest electron spin relaxation times (T1T_1T1​) at room temperature for solid-state defects are observed in nitrogen vacancy centers in diamond, which can reach 6.67 ms, and substitutional nitrogen ("P1 centers") in diamond, which exhibit a T1T_1T1​ of 2 ms. No other solid-state defect has exhibited millisecond-scale spin relaxation times at room temperature thus far. Here, we characterize the spin properties of the WAR5 defect in diamond with pulsed electron spin resonance. The observed T1T_1T1​ is one of the longest for solid-state spin defects: 0.97(27) ms at room temperature and 14.38(19) min at 4 K. The observed coherence time (T2T_2T2​) is 246(7) μμμs, which can be extended to 6.49(34) ms at 4 K with dynamical decoupling. Furthermore, we demonstrate optical spin polarization with a range of wavelengths from 405 nm to 500 nm and propose potential zero-phonon line candidates.
The nitrogen - vacancy (N-V) center is a point defect found in diamonds containing substitutional nitrogen impurities. It arises after exposure to ionizing radiation and subsequent thermal annealing. The physical structure of the center has previously been identified as a substitutional nitrogen atom located adjacent to a neutral carbon vacancy, but prior to this work knowledge of its electronic structure was very incomplete. The results presented here are intended to establish the energy level structure of the N-V center unambiguously, using nonlinear laser spectroscopy in concert with paramagnetic resonance experiments. A new technique which achieves sub-Hertz resolution in nearly degenerate four-wave mixing (NDFWM) and optical two-beam coupling experiments was applied to determine the decay rates of excited states in the N-V center. Laser-enhanced EPR experiments were performed to assign spin character to the ground state. Fluorescent emission of the center was used to determine excited state energies. In particular, these results resolve earlier conflicting reports of the N-V ground state structure and offer a picture of state energies and dynamics consistent with all observations to date. The principal results of this thesis may be summarized as follows. We show that the ground state of the center consists of a spin triplet ground state with a zero-field splitting of 2.88 GHz and a spin-lattice relaxation time of 1.170 ±\pm± 0.003 ms. The first parity-allowed transition occurs to a triplet excited state at 1.944 eV with a lifetime of 13.3 ±\pm± 0.2 ns. The first metastable singlet excited state is shown to have a lifetime of 265.3 ±\pm± 0.6 ms at room temperature and its temperature dependence measured between 77 and 295 K. Through low temperature studies the mechanism for ground state spin-lattice relaxation is determined to be a two-phonon process involving 63 meV optical phonons. Finally, the origin of satellite lines in the persistent hole-burning spectrum is tentatively explained using our picture of the energy level structure and used to infer a zero-field spin splitting in the excited triplet state of 0.6 GHz.
Nitrogen-vacancy (NV) complex in diamond is one of the most prominent solid state defects as the negatively charged NV defect (NV−) is a leading contender for quantum technologies. In quantum information processing applications, NV− is photoexcited that often leads to photoionization to neutral NV defect, NV0, and re-ionization back to NV− should occur to control the S=1 spin of NV−. As a consequence, understanding the photophysics of NV0 is crucial for controlling NV−. Furthermore, recent studies have shown that the S=1/2 electron spin of NV0 can also be initialized and read out at certain conditions that turns single NV0 a potential quantum bit. Quantum optics protocols rest on detailed knowledge on the electronic structure of the given system, which is obviously missing for NV0 in diamond. In this study, we combine the group theory and density functional theory calculations toward exploring the nature of the ground and excited states of NV0. We show that the effective three-electron system of NV0 leads to high correlation effects that make this system very challenging for ab initio simulations.